Glasses for Nuclear Waste Immobilization. Effect of Lutetium Addition on Yttrium Aluminosilicate Glass Crystallization Kinetics

Glasses have emerged as alternative materials that can be used for long-term treatment and management of radioactive waste. Specifically, glasses can be used as a matrix to immobilize the radioactive material. Within the glass industry, silicate glasses are the most widely used due to their properties and to the large knowledge existent about them. Alkaline free silicate glasses are particularly corrosion resistant. Due to the latter, rare earth aluminosilicate glasses are good candidates for actinides immobilization, especially, yttrium aluminosilicate (YAS) glasses. The crystallization kinetics of YAS glasses on heating has been already studied, and this work is focused on the effect of lutetium addition on the YAS glass crystallization kinetics. The presence of a small amount of lutetium in a YAS glass decreases the surface density of nucleation sites (Ns) by about 1 order of magnitude and significantly decreases the crystal growth rate (U). In this work, it was observed that lutetium additions on the order of 0.2 (wt %) to a YAS glass dramatically decreased Ns, for example, at 1000 °C from 1011 to 109 nuclei/m2. Additionally, U for yttrium disilicate phase decreased from (8.21 ± 0.28) μm/h to (0.54 ± 0.04) μm/h at the same temperature.

Sintering Kinetics of an Yttrium Aluminosilicate Glass

ABSTRACTYttrium aluminosilicate (YAS) glasses have been proposed as host matrices for the immobilization of radioactive elements. In addition, yttrium has been used to simulate actinides [1]. It is well known that these glasses are resistant to water corrosion and exhibit high Tg and good mechanical properties [2]. As shown in [3], on heating, yttrium disilicate and mullite / sillimanite crystals grow from the pre-existing nucleation sites on the surface, until each glass particle volume is fully crystallized (volume-homogeneous nucleation was not observed), decreasing the glassy surface available for sintering by viscous flow. Sintering takes place simultaneously, by viscous flow but competes with surface crystallization; thus, if thermal treatment is not carefully designed a vitroceramic is obtained. In this paper we study the isothermal sintering kinetics of a YAS glass-powder-size distribution and non-isothermal sintering kinetics at 1, 3, 5, 10 and 15 K/min of two YAS glass-powder-size distributions. From the experimental evidence obtained, and crystallization data from [3], we design a sintering procedure in order to achieve a high-density glass monolith with submicrometric crystalline phases.